Neutron resonances in planar waveguides

Results of experimental investigations of a neutron resonances width in planar waveguides using the time-of-flight reflectometer REMUR of the IBR-2 pulsed reactor are reported and comparison with theoretical calculations is presented. The intensity of the neutron microbeam emitted from the waveguide edge was registered as a function of the neutron wavelength and the incident beam angular divergence. The possible applications of this method for the investigations of layered nanostructures are discussed

Orbital ice: an exact Coulomb phase on the diamond lattice

We demonstrate the existence of orbital Coulomb phase as the exact ground state of p-orbital exchange Hamiltonian on the diamond lattice. The Coulomb phase is an emergent state characterized by algebraic dipolar correlations and a gauge structure resulting from local constraints (ice rules) of the underlying lattice models. For most ice models on the pyrochlore lattice, these local constraints are a direct consequence of minimizing the energy of each individual tetrahedron. On the contrary, the orbital ice rules are emergent phenomena resulting from the quantum orbital dynamics. We show that the orbital ice model exhibits an emergent geometrical frustration by mapping the degenerate quantum orbital ground states to the spin-ice states obeying the 2-in-2-out constraints on the pyrochlore lattice. We also discuss possible realization of the orbital ice model in optical lattices with p-band fermionic cold atoms.Comment: 6 pages, 5 figure

Numerical calculation of the combinatorial entropy of partially ordered ice

Using a one-parameter case as an example, we demonstrate that multicanonical simulations allow for accurate estimates of the residual combinatorial entropy of partially ordered ice. For the considered case corrections to an (approximate) analytical formula are found to be small, never exceeding 0.5%. The method allows one as well to calculate combinatorial entropies for many other systems.Comment: Extended version: 7 pages, 10 figures (v1 is letter-type version

Magnetic charge and ordering in kagome spin ice

We present a numerical study of magnetic ordering in spin ice on kagome, a two-dimensional lattice of corner-sharing triangles. The magnet has six ground states and the ordering occurs in two stages, as one might expect for a six-state clock model. In spin ice with short-range interactions up to second neighbors, there is an intermediate critical phase separated from the paramagnetic and ordered phases by Kosterlitz-Thouless transitions. In dipolar spin ice, the intermediate phase has long-range order of staggered magnetic charges. The high and low-temperature phase transitions are of the Ising and 3-state Potts universality classes, respectively. Freeze-out of defects in the charge order produces a very large spin correlation length in the intermediate phase. As a result of that, the lower-temperature transition appears to be of the Kosterlitz-Thouless type.Comment: 20 pages, 12 figures, accepted version with minor change

Entropy-based measure of structural order in water

We analyze the nature of the structural order established in liquid TIP4P water in the framework provided by the multi-particle correlation expansion of the statistical entropy. Different regimes are mapped onto the phase diagram of the model upon resolving the pair entropy into its translational and orientational components. These parameters are used to quantify the relative amounts of positional and angular order in a given thermodynamic state, thus allowing a structurally unbiased definition of low-density and high-density water. As a result, the structurally anomalous region within which both types of order are simultaneously disrupted by an increase of pressure at constant temperature is clearly identified through extensive molecular-dynamics simulations.Comment: 5 pages, 2 figures, to appear in Phys. Rev. E (Rapid Communication

Benchmarking acid and base dopants with respect to enabling the ice V to XIII and ice VI to XV hydrogen-ordering phase transitions

Doping the hydrogen-disordered phases of ice V, VI and XII with hydrochloric acid (HCl) has led to the discovery of their hydrogen-ordered counterparts ices XIII, XV and XIV. Yet, the mechanistic details of the hydrogen-ordering phase transitions are still not fully understood. This includes in particular the role of the acid dopant and the defect dynamics that it creates within the ices. Here we investigate the effects of several acid and base dopants on the hydrogen ordering of ices V and VI with calorimetry and X-ray diffraction. HCl is found to be most effective for both phases which is attributed to a favourable combination of high solubility and strong acid properties which create mobile H3O+ defects that enable the hydrogen-ordering processes. Hydrofluoric acid (HF) is the second most effective dopant highlighting that the acid strengths of HCl and HF are much more similar in ice than they are in liquid water. Surprisingly, hydrobromic acid doping facilitates hydrogen ordering in ice VI whereas only a very small effect is observed for ice V. Conversely, lithium hydroxide (LiOH) doping achieves a performance comparable to HF-doping in ice V but it is ineffective in the case of ice VI. Sodium hydroxide, potassium hydroxide (as previously shown) and perchloric acid doping are ineffective for both phases. These findings highlight the need for future computational studies but also raise the question why LiOH-doping achieves hydrogen-ordering of ice V whereas potassium hydroxide doping is most effective for the 'ordinary' ice Ih.Comment: 18 pages, 7 figures, 1 tabl

The thickness of a liquid layer on the free surface of ice as obtained from computer simulation

Molecular dynamic simulations were performed for ice Ih with a free surface by using four water models, SPC/E, TIP4P, TIP4P/Ice and TIP4P/2005. The behavior of the basal plane, the primary prismatic plane and of the secondary prismatic plane when exposed to vacuum was analyzed. We observe the formation of a thin liquid layer at the ice surface at temperatures below the melting point for all models and the three planes considered. For a given plane it was found that the thickness of a liquid layer was similar for different water models, when the comparison is made at the same undercooling with respect to the melting point of the model. The liquid layer thickness is found to increase with temperature. For a fixed temperature it was found that the thickness of the liquid layer decreases in the following order: the basal plane, the primary prismatic plane, and the secondary prismatic plane. For the TIP4P/Ice model, a model reproducing the experimental value of the melting temperature of ice, the first clear indication of the formation of a liquid layer appears at about -100 Celsius for the basal plane, at about -80 Celsius for the primary prismatic plane and at about -70 Celsius for the secondary prismatic plane.Comment: 41 pages and 13 figure

Energy benchmarks for water clusters and ice structures from an embedded many-body expansion

We show how an embedded many-body expansion (EMBE) can be used to calculate accurate \emph{ab initio} energies of water clusters and ice structures using wavefunction-based methods. We use the EMBE described recently by Bygrave \emph{et al.} (J. Chem. Phys. \textbf{137}, 164102 (2012)), in which the terms in the expansion are obtained from calculations on monomers, dimers, etc. acted on by an approximate representation of the embedding field due to all other molecules in the system, this field being a sum of Coulomb and exchange-repulsion fields. Our strategy is to separate the total energy of the system into Hartree-Fock and correlation parts, using the EMBE only for the correlation energy, with the Hartree-Fock energy calculated using standard molecular quantum chemistry for clusters and plane-wave methods for crystals. Our tests on a range of different water clusters up to the 16-mer show that for the second-order M\o{}ller-Plesset (MP2) method the EMBE truncated at 2-body level reproduces to better than 0.1 m$E_{\rm h}$/monomer the correlation energy from standard methods. The use of EMBE for computing coupled-cluster energies of clusters is also discussed. For the ice structures Ih, II and VIII, we find that MP2 energies near the complete basis-set limit reproduce very well the experimental values of the absolute and relative binding energies, but that the use of coupled-cluster methods for many-body correlation (non-additive dispersion) is essential for a full description. Possible future applications of the EMBE approach are suggested

Free energy landscapes for homogeneous nucleation of ice for a monatomic water model

We simulate the homogeneous nucleation of ice from supercooled liquid water at 220 K in the isobaric-isothermal ensemble using the MW monatomic water potential. Monte Carlo simulations using umbrella sampling are performed in order to determine the nucleation free energy barrier. We find the Gibbs energy profile to be relatively consistent with that predicted by classical nucleation theory; the free energy barrier to nucleation was determined to be ~18 kT and the critical nucleus comprised ~85 ice particles. Growth from the supercooled liquid gives clusters that are predominantly cubic, whilst starting with a pre-formed subcritical nucleus of cubic or hexagonal ice results in the growth of predominantly that phase of ice only.Comment: 11 pages, 6 figures; updated with nucleation rates and additional comparisons with some newly published paper